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Roh, Joo Yeon; Smith, Matthew D.; Crane, Matthew J.; Biner, Daniel; Milstein, Tyler J.; Krämer, Karl; Gamelin, Daniel R.

doi:10.1103/physrevmaterials.4.105405

Cited by 37 publications

(57 citation statements)

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“…In this mechanism, the Ln 3+ ion or ions form shallow dopant-induced defects states that either act as electron traps or are eventually reduced energetically allowed. We do not have proof that the first step of the photosensitization is electron transfer to a defect-incorporated Ln 3+ , but others 10,11,27 have linked the involvement of the trap state, which includes two lanthanide ions, to the ability of the host to simultaneously sensitize two Yb 3+ ions. The system starts in the ground state, NC-(Ln 3+ -Cl − -V Pb 2− -Cl − -Ln 3+ ), where V Pb 2− denotes a lead vacancy.…”

Section: ■ Results and Discussionmentioning

confidence: 80%

“…10,22,24 Upon Ln 3+ incorporation, a new sub-picosecond time component (which we denote as τ 1 ) was observed for all species regardless of the degree of band-edge PL quenching or enhancement. Based on previous reports, 10,11 we assign τ 1 to electron trapping by a specific defect surrounding a lead vacancy (V Pb 2− ) with the structure Ln 3+ -Cl − -V Pb 2− -Cl − -Ln 3+ ; this defect is known as a McPherson pair. 25 Several reports show that shallow electron traps, such as the aliovalent dopant-induced defects we propose to have here, increase the band-edge PL of the host by protecting the conduction band electrons from deep traps while allowing them to de-trap to radiative states.…”

Section: ■ Results and Discussionmentioning

confidence: 98%

“…9 Pan et al 6 implicated defects in the lattice of CsPbCl 3 NCs as electron traps that mediate nonradiative energy transfer from the NC exciton to the Ln 3+ ion to form the emissive species. The role of defects in photosensitization was further specified by Milstein et al 10 and Roh et al, 11 who showed that shallow defect sites containing two proximate Yb 3+ within Yb 3+ -doped CsPbCl 3 NCs depopulate the NC conduction band within picoseconds. That study also implicated these defects as intermediates for simultaneous energy transfer to both ions, resulting in a quantum cutting process and >100% emission quantum yield from the NC.…”

Section: ■ Introductionmentioning

confidence: 95%

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Photoredox-Mediated Sensitization of Lanthanide Dopants by Perovskite Nanocrystals

et al. 2021

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Trivalent lanthanide ions (Ln3+) have electronically isolated f-orbitals that support excited states, which, due to their ultra-narrow emission and long spin coherence lifetimes, are potentially suitable as hosts for spin qubits. These excited states must however be generated through photosensitization due to the low-absorption cross sections of Ln3+. This paper describes the mechanism of photosensitization of Yb3+ and Sm3+ ions by their CsPbCl3 perovskite nanocrystal (NC) host matrices, through examination of the photophysical processes in NCs doped with seven different Ln3+ ions. An observed dependence of the NC’s band-edge photoluminescence (PL) on the potential of the Ln3+/Ln2+ redox couple implies the presence of a charge transfer intermediate in the sensitization mechanism. Ultrafast transient absorption (TA) experiments indicate that (i) a previously identified Ln3+-Cl–-VPb 2–-Cl–-Ln3+ defect is formed within 1 ps of photoexcitation of the NC regardless of the yield of photosensitization, (ii) the first step of photosensitization, an electron transfer, occurs in 10s of picoseconds, and (iii) the resulting charge-separated state forms the emissive species, Ln3+*, through a slower subsequent hole transfer from the NC. A mechanistic understanding of Ln3+ dopant sensitization provides a framework for choosing the right combination of host matrix and Ln3+ species for efficient photosensitization.

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Section: ■ Results and Discussionmentioning

confidence: 80%

Section: ■ Results and Discussionmentioning

confidence: 98%

Section: ■ Introductionmentioning

confidence: 95%

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Photoredox-Mediated Sensitization of Lanthanide Dopants by Perovskite Nanocrystals

et al. 2021

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“…In the spot-lighted paper (Roh et al, 2020), J.Y. Diana Roh and others investigate the fundamental origins of down-conversion-also known as quantum cutting-in depth.…”

Section: Spot Light In Light Sources and Luminescent Materialsmentioning

confidence: 99%

mentioning

confidence: 99%

Frontiers in Photonics Spot Light

et al. 2022

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Realization of 1.54‐µm Light‐Emitting Diodes Based on Er³⁺/Yb³⁺Co‐Doped CsPbCl₃ Films

Liu

Zhou

et al. 2023

Advanced Materials

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Erbium ions (Er 3+ , 1.54 μm) electric pumped light sources with excellent optical properties and a simple fabrication process are urgently desired to satisfy the development of silicon-based integration photonics. The previous Er-based electroluminescence devices are mainly based on Er-complexes or Er-doped oxide compounds, which usually suffer from low external quantum efficiency(EQE)or high applied voltage etc. In this work, a novel type of Er 3+ /Yb 3+ co-doped lead-halide perovskite films (Er 3+ /Yb 3+ :CsPbCl 3 ) with the maximum photoluminescence quantum yield of 30.12% are prepared by a simple two-step solution-coating method and the corresponding light emitting diodes (Er-PeLEDs) are fabricated, which demonstrate an almost pure 1.54-μm emission and a peak EQE up to 0.366% at a low applied voltage of 1.4 V. Strong negative thermal quenching effect may help Er-PeLEDs suppress Joule heating quenching. These excellent LED properties benefit mainly from the outstanding regulatory performance of acetate to perovskite films, the excellent semiconductor behavior and strong ionic property of the perovskite, and the involvement of Yb 3+ ions, which can directly and efficiently transfer the exciton energy to Er 3+ through a quantum cutting process. Overall, the realization of 1.54-μm Er-PeLEDs offers new opportunities for silicon-based integrated light sources.

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Yb3+ speciation and energy-transfer dynamics in quantum-cutting Yb3+ -doped <

Cited by 37 publications

References 50 publications

Photoredox-Mediated Sensitization of Lanthanide Dopants by Perovskite Nanocrystals

Photoredox-Mediated Sensitization of Lanthanide Dopants by Perovskite Nanocrystals

Frontiers in Photonics Spot Light

Realization of 1.54‐µm Light‐Emitting Diodes Based on Er³⁺/Yb³⁺Co‐Doped CsPbCl₃ Films

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Yb3+ speciation and energy-transfer dynamics in quantum-cutting Yb3+ -doped <

Cited by 37 publications

References 50 publications

Photoredox-Mediated Sensitization of Lanthanide Dopants by Perovskite Nanocrystals

Photoredox-Mediated Sensitization of Lanthanide Dopants by Perovskite Nanocrystals

Frontiers in Photonics Spot Light

Realization of 1.54‐µm Light‐Emitting Diodes Based on Er3+/Yb3+Co‐Doped CsPbCl3 Films

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Realization of 1.54‐µm Light‐Emitting Diodes Based on Er³⁺/Yb³⁺Co‐Doped CsPbCl₃ Films